In accordance with the present invention, there are prepared two-dimensional polymers from monomers that satisfy the following three conditions: (1) they react in ordered configurations, (2) they have more than one reactive group, and (3) they have at least one terminus free of reactive groups. The monomers useful in the invention contain polymerizable, e.g., acrylate, groups and chiral functions, e.g., nitrile, that can undergo rapid thermal polymerization in the isotropic molten state to yield a product which forms smectic phases of high thermal stability. Based on spectroscopic evidence, phase behavior, and solubility characteristics, the reaction products are two-dimensional polymers which can be described as molecular sheets. The two-dimensional polymers form because two independent polymerization reactions can be thermally activated among the monomers in locally ordered configurations. These ordered configurations result from the aggregation or alignment of monomers by molecular recognition. If only a single polymerization reaction were to occur, a "comb" polymer, i.e., a single backbone polymer chain having pendent side chains, and not a two-dimensional polymer, would form. On the other hand, if both polymerizations were activated among monomers in disordered configurations, the product of the reaction would be an insoluble crosslinked gel. Also, if both reactive chemical functions were situated at the termini of the monomer molecules, the product would also be a crosslinked, three-dimensional gel.